The interaction between light and plasmonic metal nanostructures has fascinated mankind ever since Faraday’s discovery of the ruby-red color of colloidal gold in the mid-1800s. This phenomenon naturally arises from collective many-body excitations; however, our understanding of the detailed quantum-mechanical mechanisms in these collective excitations is severely limited due to the sheer size and complexity of plasmonic nanostructure-molecule interfaces (cf. Fig. 1). Specifically, while classical electrodynamics methods can handle metallic nanostructures at a continuum level, they cannot provide a predictive, first-principles-based description of plasmonic systems at the quantum level. At the other extreme, conventional linear-response time-dependent methods can probe the true quantum nature of chemical systems; however, these methods cannot tackle the large sizes relevant to collective excitations in plasmonic materials. To bridge this immense knowledge gap, this OpenEye COMP poster presentation will describe my group’s recent progress in developing efficient quantum computational methods and GPU enhancements to probe real-time plasmonic excitations in large metallic plasmonic systems and arrays. Specifically, we have developed and utilized a new real-time, time-dependent density functional tight binding (RT-TDDFTB) computational approach to efficiently and accurately probe the electron dynamics in both metallic nanocluster-molecule and nanocluster-array systems. Most importantly, the RT-TDDFTB approaches utilized in our research bridges the gap between continuum-level approaches and extremely small, first-principles-based calculations for exploring collective plasmonic excitations – all carried out on the same footing at a quantum-mechanical level.

Accelerating real-time electron dynamics calculations of large plasmonic systems

253rd National Meeting (2017)

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